CN105792914A - Cold start catalyst and its use in exhaust systems - Google Patents

Cold start catalyst and its use in exhaust systems Download PDF

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Publication number
CN105792914A
CN105792914A CN201480066543.1A CN201480066543A CN105792914A CN 105792914 A CN105792914 A CN 105792914A CN 201480066543 A CN201480066543 A CN 201480066543A CN 105792914 A CN105792914 A CN 105792914A
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CN
China
Prior art keywords
catalyst
molecular sieve
cooled activated
activated catalyst
base material
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CN201480066543.1A
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Chinese (zh)
Inventor
H-Y·陈
R·R·拉什拉姆
刘东霞
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Johnson Matthey PLC
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Johnson Matthey PLC
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Application filed by Johnson Matthey PLC filed Critical Johnson Matthey PLC
Priority to CN202211131732.5A priority Critical patent/CN115430458A/en
Publication of CN105792914A publication Critical patent/CN105792914A/en
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    • B01J29/66—Crystalline aluminosilicate zeolites; Isomorphous compounds thereof of the ferrierite type, e.g. types ZSM-21, ZSM-35 or ZSM-38, as exemplified by patent documents US4046859, US4016245 and US4046859, respectively containing iron group metals, noble metals or copper
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    • B01J29/85—Silicoaluminophosphates [SAPO compounds]
    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F01—MACHINES OR ENGINES IN GENERAL; ENGINE PLANTS IN GENERAL; STEAM ENGINES
    • F01N—GAS-FLOW SILENCERS OR EXHAUST APPARATUS FOR MACHINES OR ENGINES IN GENERAL; GAS-FLOW SILENCERS OR EXHAUST APPARATUS FOR INTERNAL COMBUSTION ENGINES
    • F01N2410/00—By-passing, at least partially, exhaust from inlet to outlet of apparatus, to atmosphere or to other device
    • F01N2410/06—By-passing, at least partially, exhaust from inlet to outlet of apparatus, to atmosphere or to other device at cold starting
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Abstract

A cold start catalyst is disclosed. The cold start catalyst is effective to adsorb NO<x> and hydrocarbons (HC) at or below a low temperature and to covert and release the adsorbed NO<x> and HC at temperatures above the low temperature. The cold start catalyst comprises a molecular sieve catalyst and a supported platinum group metal catalyst. The molecular sieve catalyst consists essentially of a noble metal and a molecular sieve. The supported platinum group metal catalyst comprises one or more platinum group metals and one or more inorganic oxide carriers. The invention also includes an exhaust system comprising the cold start catalyst, and a method for treating exhaust gas from an internal combustion engine utilizing the cold start catalyst.

Description

Cooled activated catalyst and its purposes in gas extraction system
Invention field
The present invention relates to cooled activated catalyst and it is for the purposes in the gas extraction system of internal combustion engine.
Background of invention
Internal combustion engine creates the waste gas comprising various pollutant, including nitrogen oxides (" NOx"), carbon monoxide and unburned hydrocarbon, this is the theme of government legislation.Emission control systems is widely used for reducing the amount of these pollutant being discharged into air, once they reach its operation temperature (being generally 200 DEG C and higher), generally obtains very high efficiency.But, it is relative inefficiencies that these systems operate temperature (" cold start-up " period) lower than it.
From the amount of diesel oil or the pollutant of gasoline engine emissions, the challenge that discharge becomes main can be reduced during cold start-up along with even tightened up country and regional legislation reduce.Therefore, for reducing the NO of discharge in cold start processxContinue to be explored with the method for the level of hydrocarbon.
Cold start-up hydrocarbon is controlled, has investigated the hydrocarbon catch parts based on zeolite.In such systems, zeolite adsorption and store hydrocarbon during starting, when delivery temperature sufficiently high with desorption hydrocarbon time, the hydrocarbon that is stored of release.Then, when downstream catalytic component reaches its operation temperature, the hydrocarbon of desorption is converted.
For cold start-up NOxControl, particularly in, under lean-burn condition, have studied NOxStore and release catalyst.Catalyst Adsorption NO during heating upxWith at higher delivery temperature thermal desorption NOx.Downstream catalyst such as SCR (" SCR ") or NOxAdsorption catalyst (" NAC ") is effectively by the NO of desorptionxIt is reduced to nitrogen.
Generally, NOxSorbent material is made up of the inorganic oxide being coated with at least one platinum group metal such as aluminium oxide, silicon dioxide, ceria, zirconium oxide, titanium dioxide or mixed oxide.PCT international application WO2008/047170 discloses a kind of system, wherein from the NO of lean exhaust gasxAt the temperature adsorption lower than 200 DEG C with then higher than 200 DEG C of thermal desorptions.Instruction NOxAdsorbent is made up of palladium and cerium oxide or mixed oxide or mixed oxide or composite oxides containing cerium and other transition metal at least one.
PCT international application WO2004/076829 discloses exhaust gas purification system, it NO including being arranged on SCR catalyst upstreamxStore catalyst.NOxStore catalyst to comprise with at least one platinum group metal (Pt, Pd, Rh, or Ir) coating or at least one alkali metal of activation, alkaline-earth metal or rare earth metal.Instruct particularly preferred NOxStore catalyst comprise with platinum coating cerium oxide and this external based on the platinum on the carrier of aluminium oxide as oxidation catalyst.EP1027919 discloses NOxSorbent material, it comprises porous carrier materials, for instance aluminium oxide, zeolite, zirconium oxide, titanium dioxide, and/or lanthana, and the noble metal (Pt, Pd, and/or Rh) of at least 0.1wt%.For load platinum on alumina.
Additionally, US patent No.5,656,244 and 5,800,793 describe combination NOxThe system of storage/release catalyst and three-way catalyst.Instruction NOxAdsorbent comprises the oxide of chromium, copper, nickel, manganese, molybdenum or cobalt (except other metal), and its load is on aluminium oxide, mullite, cordierite or carborundum.PCT international application WO03/056150 describes combination low temperature NO2The system of material for trapping and soot filter.Instruction low temperature NO2Material for trapping comprises the zeolite with alkali metal cation-exchanged, its mesolite is selected from ZSM-5, ETS-10, Y-zeolite, β zeolite, ferrierite, modenite, titanium silicate and aluminum phosphate and base metal, and it is selected from Mn, Cu, Fe, Co, W, Re, Sn, Ag, Zn, Mg, Li, Na, K, Cs, Nd and Pr.
Unfortunately, particularly in high NOxUnder efficiency of storage, the NO of this systemxAbsorbability is not sufficiently high.Because the control of increasingly stringent is discharged into the NO of air by internal combustion enginexMake laws with the whole world of the amount of hydrocarbon, be constantly present the needs for exhaust gas cleaning significantly more efficient during cold start.In order to overcome these problems, the open No.2012/0308439A1 of U. S. application instructs cooled activated catalyst, it comprises (1) and comprises the zeolite catalyst of base metal, noble metal and zeolite, and (2) comprise the platinum metal catalysts of one or more platinums group metal and the load of one or more inorganic oxide carriers.But, the open No.2012/0308439A1 of U. S. application needs the base metal of zeolite catalyst components.
For any automotive system and method, it is desirable to obtain in exhaust treatment system and still further improve, particularly in cold start conditions.A kind of offer new cooled activated catalyst from the cleaning of the enhancing of the waste gas of internal combustion engine is provided.
Summary of the invention
The present invention is for being effective in absorption NO below certain low temperaturexWith hydrocarbon (HC) and higher than described low temperature temperature inversion and release absorption NOxCooled activated catalyst with HC.Cooled activated catalyst comprises the platinum metal catalysts of molecular sieve catalyst and load.Molecular sieve catalyst is substantially made up of noble metal and molecular sieve.The platinum metal catalysts of load comprises one or more platinums group metal and one or more inorganic oxide carriers.Present invention additionally comprises a kind of gas extraction system including cooled activated catalyst and a kind of method utilizing cooled activated catalyst to process the waste gas from internal combustion engine.The cooled activated catalyst NO by improvingxStore and NOxThe CO oxidation that the hydrocarbon convert, improved stores and converts and improves is effectively reduced discharge during cold start-up.
Detailed description of the invention
The cooled activated catalyst of the present invention comprises the platinum metal catalysts of molecular sieve catalyst and load.Cooled activated catalyst is effective in absorption NO below certain low temperaturexWith hydrocarbon (HC) and higher than described low temperature temperature inversion and release absorption NOxAnd HC.Preferably, low temperature is about 200 DEG C.Molecular sieve catalyst is substantially made up of noble metal and molecular sieve, and is preferably made up of noble metal and molecular sieve.Noble metal is preferably palladium, platinum, rhodium, gold, silver, iridium, ruthenium, osmium or its mixture；It is more preferably palladium, platinum, rhodium or its mixture.Palladium is particularly preferred.
Molecular sieve can be any naturally occurring or synthetic molecular sieve, including zeolite, and is preferably made up of aluminum, silicon and/or phosphorus.Molecular sieve is generally of the SiO shared and connect by oxygen atom4、AlO4And/or PO4Three-dimensional setting but it also may for two-dimensional structure.Framework of molecular sieve is generally anionic, and it is balanced by charge compensating cations, is generally alkali and alkaline earth element (such as, Na, K, Mg, Ca, Sr, and Ba), ammonium ion and proton.
Molecular sieve is preferably up to the small pore molecular sieve that ring size is 8 Tetrahedral atoms, and maximum loop is of a size of the mesoporous molecular sieve of 10 Tetrahedral atoms, or maximum loop is of a size of the large pore molecular sieve of 12 Tetrahedral atoms.It is highly preferred that molecular sieve has the framing structure of AEI, MFI, EMT, ERI, MOR, FER, BEA, FAU, CHA, LEV, MWW, CON, EUO or its mixture.
Molecular sieve catalyst can be prepared by any of mode.Such as, noble metal can be added into molecular sieve to form molecular sieve catalyst by any of mode, and the mode of interpolation is not considered as particularly critical.Such as, precious metal chemical complex (such as Palladous nitrate .) can be exchanged by dipping, absorption, ion, just wet, be precipitated even load over a molecular sieve.
The platinum metal catalysts of load comprises one or more platinums group metal (" PGM ") and one or more inorganic oxide carriers.PGM can be platinum, palladium, rhodium, iridium or its combination, and most preferably platinum and/or palladium.Inorganic oxide carrier most commonly includes the oxide of the 2nd, 3,4,5,13 and 14 race's elements.Useful inorganic oxide carrier preferably has 10-700m2The surface area of/g, the pore volume of 0.1-4mL/g, peace treatyAperture.Inorganic oxide carrier is preferably aluminium oxide, silicon dioxide, titanium dioxide, zirconium oxide, ceria, niobium oxide, tantalum pentoxide, molybdenum oxide, tungsten oxide, or its any two or more kinds of mixed oxides or composite oxides, for instance silica-alumina, ceria-zirconia or alumina-ceria-zirconium oxide.Aluminium oxide and ceria are particularly preferred.
The platinum metal catalysts of load can be prepared by any of mode.Preferably, one or more platinums group metal are loaded to form the PGM catalyst of load on one or more inorganic oxides by any of mode, and the mode of interpolation is not considered as particularly critical.Such as, platinum compounds (such as platinum nitrate) can be exchanged by dipping, absorption, ion, just wet, be precipitated even load on inorganic oxide.Other metal such as ferrum, manganese, cobalt and barium can also be added into the PGM catalyst of load.
The cooled activated catalyst of the present invention can be prepared by means commonly known in the art.The platinum metal catalysts of molecular sieve catalyst and load can physical mixed to produce cooled activated catalyst.Preferably, cooled activated catalyst farther includes flow through substrate or filtering type base material.In one embodiment, the platinum metal catalysts of molecular sieve catalyst and load is coated on flow type or filtering type base material, and carrier coating program is preferably used is deposited on flow type or filtering type base material to produce cooled activated catalyst system.
Flow type or filtering type base material are able to comprise the base material of catalyst component.Base material is preferably ceramic base material or metal base.Ceramic base material can be made up of any applicable refractory material, for instance, aluminium oxide, silicon dioxide, titanium dioxide, ceria, zirconium oxide, magnesium oxide, zeolite, silicon nitride, carborundum, zirconium silicate, magnesium silicate, aluminosilicate, metal aluminosilicates (such as cordierite and spodumene), or its any two or more kinds of mixture or mixed oxide.Cordierite, zeopan and carborundum are particularly preferred.
Metal base can be made up of any applicable metal, and particularly heat-resisting metal and metal alloy such as titanium and rustless steel and containing ferrum, nickel, chromium and/or aluminum (except other trace metal) Alfer.
Flow through substrate is preferably the flow type material all in one piece with alveolate texture, and described alveolate texture has multiple little, parallel thin-walled channels, and it runs through extension axially across base material and from entrance or the outlet of base material.The channel cross-section of base material can be any shape, but preferred square, sinusoidal, triangle, rectangle, hexagon, trapezoidal, circular or oval.
Filtering type base material is preferably wall flow monolith filter.The passage of wall-flow filter is alternately closed, and this allows exhaust gas stream to enter passage from entrance, then passes through conduit wall, and leaves filter from the different passages leading to outlet.Therefore, the granule in exhaust gas stream is captured in the filter.
The platinum group catalyst of molecular sieve catalyst and load can be added into flow type or filtering type base material by any of mode.Carrier coating program is used to prepare the exemplary process of cooled activated catalyst as mentioned below.It will be appreciated that method hereafter can change according to different embodiment of the present invention.And, the order being added on by the PGM catalyst of molecular sieve catalyst and load on flow type or filtering type base material is not considered as key.Therefore, molecular sieve catalyst can be coated on base material by carrier before the PGM catalyst of load, or the PGM catalyst of load can be coated on base material by carrier before molecular sieve catalyst.
The molecular sieve catalyst of preforming can be added into flow type or filtering type base material by carrier coating step.Alternatively, molecular sieve catalyst can be formed on the substrate by the base material being coated in by unmodified molecular sieve first carrier on flow type or filtering type base material to produce molecular sieve coating.It is then possible to noble metal is added into the base material of molecular sieve coating, this can pass through impregnating process etc. and complete.
Carrier coating program is carried out to form slurry preferably by molecular sieve catalyst (or the unmodified molecular sieve) granule that first pulp is segmented in appropriate solvent (preferred water).Additional component such as binding agent or stabilizer can also introduce slurry as the mixture of water solublity or dispersible compounds.Slurry preferably comprises the solid of 10-70 weight %, more preferably 20-50 weight %.Before forming slurry, molecular sieve catalyst (or unmodified molecular sieve) granule preferably is subjected to size reduction and processes (such as, grinding) so that the particle mean size of solid particle is that diameter is less than 20 microns.
Then, flow type or filtering type base material can immerse slurry or slurry can be coated on base material by one or many so that wish that the depositing catalytic material of load capacity is on base material.If noble metal introduces molecular sieve before not being coated with flow type or filtering type base material at carrier, the base material of molecular sieve coating is generally dry and calcines, then noble metal can be added into the base material of molecular sieve coating by any of mode, including dipping, absorption or ion exchange, such as, precious metal chemical complex (such as Palladous nitrate .) is utilized.Preferably, the whole length slurry of flow type or filtering type base material is coated with so that molecular sieve catalyst carrier coating covers the whole surface of base material.
Flow type or filtering type base material with the coating of molecular sieve catalyst slurry and with precious metal impregnation (the need to) after, coated base material is preferably dry and then passes through and calcines at the heating temperatures raised to form the base material that molecular sieve catalyst is coated with.Preferably, calcining carries out about 1-8 hour at 400-600 DEG C.
Add to the carrier coating completing the PGM catalyst of load preferably by first preparing the PGM catalyst granules of load of the segmentation slurry in appropriate solvent (preferred water).Before forming slurry, the PGM catalyst granules of load preferably is subjected to size reduction and processes (such as, grinding) so that the particle mean size of solid particle is that diameter is less than 20 microns.Additional component such as transition metal oxide, binding agent, stabilizer or accelerator can introduce in slurry as water dispersible or water soluble compound.
Then the base material of molecular sieve catalyst coating can immerse the PGM catalyst pulp of the PGM catalyst pulp of load or load and can be coated on the base material of molecular sieve catalyst coating by one or many so that wish that the depositing catalytic material of load capacity is on base material.
Alternatively, the slurry only comprising inorganic oxide can be first deposited upon on the base material of molecular sieve catalyst coating to form the base material of inorganic oxide coating, is dried afterwards and calcining step.Then platinum group metal is added into the base material of inorganic oxide coating by any of mode, including dipping, absorption or ion exchange platinum group metal compounds (such as platinum nitrate).
Preferably, the PGM catalyst pulp coating of the whole length load of flow type or filtering type base material, thus the carrier coating of the PGM catalyst of load covers the whole surface of base material.
After the PGM catalyst pulp of flow type or filtering type base material load is coated with, it is preferable that dry and then calcine to produce cooled activated catalyst at the heating temperatures raised.Preferably, calcining carries out about 1-8 hour at 400-600 DEG C.
In an alternative embodiment, flow type or filtering type base material comprise molecular sieve catalyst, and the platinum metal catalysts of load is coated on molecular sieve catalyst base material.In this case, molecular sieve is extruded to form flow type or filtering type base material, and the platinum metal catalysts of load is coated on molecular sieve catalyst flow type or the filtering type base material of extrusion.The base material of molecular sieve catalyst extrusion is preferably cellular flow type material all in one piece.
Molecular sieve base material and the melikaria of extrusion and prepare their method and be well known in the art.Referring to such as, U.S. Patent number 5,492,883,5,565,394, and 5,633,217 and U.S. Patent No. Re.34,804.Generally, molecular screen material mixes with durable adhesion agent such as organic siliconresin and temporary adhesive such as methylcellulose, and mixture is extruded to form honeycomb green body, and then it calcine and sinter to form final molecular sieve substrate monolith.Molecular sieve can comprise noble metal before extrusion so that noble metal/molecular sieve base material (flow type or filter) material all in one piece is produced by extrusion program.
If molecular sieve substrate monolith formed, then molecular sieve substrate monolith stand impregnating process (the need to) with by noble-metal-supported on molecular sieve material all in one piece, carry out afterwards carrier coating step with carrier be coated with load PGM catalyst.
Present invention additionally comprises the gas extraction system of internal combustion engine for including cooled activated catalyst.Gas extraction system preferably includes and one or more other can remove the after-treatment device of pollutant in normal running temperature from the waste gas of internal combustion engine.Preferably, gas extraction system includes cooled activated catalyst and one or more are selected from other following catalyst member: (1) SCR (SCR) catalyst, (2) particulate filter, (3) SCR filter, (4) NOxAdsorption catalyst, (5) three-way catalyst, (6) oxidation catalyst, or its combination any.
These after-treatment devices are well known in the art.SCR (SCR) catalyst be by with nitrogen compound (such as ammonia or carbamide) or hydrocarbon (lean combustion NOxReduction) react NOxIt is reduced to N2Catalyst.Typical SCR catalyst comprises vanadium oxide-titanium deoxide catalyst, vanadium oxide-tungsten oxide-titanium deoxide catalyst, or metal/zeolite catalyst, for instance ferrum/β zeolite, copper/β zeolite, copper/SSZ-13, copper/SAPO-34, Fe/ZSM-5, or copper/ZSM-5.
Particulate filter is the device of the granule reducing the aerofluxus from internal combustion engine.Particulate filter includes catalysed particulate filter and naked (on-catalytic) particulate filter.Catalysed particulate filter (is applied for diesel oil and gasoline) and is included metal and metal oxide component (such as Pt, Pd, Fe, Mn, Cu, and ceria) with oxygenated hydrocarbon and carbon monoxide (except destruction is by the flue dust of filter traps).
SCR filter (SCRF) is the single substrate setup of the function of combination S CR and particulate filter.They are for reducing the NO from internal combustion enginexAnd particulate emission.Except SCR catalyst is coated with, particulate filter can also include other metal and metal oxide component (such as Pt, Pd, Fe, Mn, Cu and ceria) with oxygenated hydrocarbon and carbon monoxide (except destruction is by the flue dust of filter traps).
NOxAdsorption catalyst (NAC) design to adsorb NO when lean burn exhaust gasx, under rich condition, discharge the NO of absorptionx, and the NO of reduction releasexTo form N2.NAC generally includes NOx-storage component (such as, Ba, Ca, Sr, Mg, K, Na, Li, Cs, La, Y, Pr and Nd), oxidation component (preferred Pt) and reduction components (preferred Rh).These components are included on one or more carriers.
Three-way catalyst (TWC) generally at stoichiometric conditions for petrol engine with on single device by NOxIt is converted into N2, convert carbon monoxide to CO2, and convert a hydrocarbon to CO2And H2O。
Oxidation catalyst and particularly diesel oxidation catalyst (DOC) are well known in the art.Oxidation catalyst designs so that CO is oxidized to CO2And the organic fraction (solvable organic fraction) of gas phase hydrocarbon (HC) and diesel particulate is oxidized to CO2And H2O.Typical oxidation catalyst includes the platinum on high surface area inorganic oxide supports such as aluminium oxide, silica-alumina and zeolite and optional palladium.
Gas extraction system can be constructed so that cooled activated catalyst is arranged close to electromotor and extra after-treatment device is arranged on the downstream of cooled activated catalyst.Therefore, in normal operation condition, engine exhaust first flows through cooled activated catalyst, contacts after-treatment device afterwards.Alternatively, gas extraction system can comprise valve or other means for guiding gas so that during cold start-up, (temperature lower than about 150-220 DEG C, as measured at after-treatment device place) guides exhaust gas contact after-treatment device, flow to cooled activated catalyst afterwards.Once after-treatment device reaches operation temperature (about 150-220 DEG C, as measured at after-treatment device place), then reboot useless air flow contacts cooled activated catalyst, contact after-treatment device afterwards.This guarantees that the temperature of cooled activated catalyst keeps low, continues the longer time, therefore improves the efficiency of cooled activated catalyst, allows after-treatment device to reach operation temperature quickly simultaneously.U.S. Patent No. 5,656,244 such as teaches the device controlling waste gas stream during cold start-up and normal operating condition, and the instruction of this patent is incorporated by reference into herein.
Present invention additionally comprises a kind of process method from the waste gas of internal combustion engine.The method include certain low temperature or lower than the temperature of this low temperature by NOxIt is adsorbed on cooled activated catalyst with hydrocarbon (HC), higher than NO from cooled activated catalyst of the temperature inversion of described low temperature and thermal desorptionxAnd HC, and catalysis removes the NO of desorption on the catalyst member in the downstream of cooled activated catalystxAnd HC.Preferably, low temperature is about 200 DEG C.
The catalyst member in the downstream of cooled activated catalyst is SCR catalyst, particulate filter, SCR filter, NOxAdsorption catalyst, three-way catalyst, oxidation catalyst or its combination.
Below example only describes the present invention.It would be recognized by those skilled in the art that the multiple modification in present invention spirit and right.
Embodiment 1: the preparation of catalyst
Comparative catalyst 1A:Pd-Fe/ β zeolite+Pt/Al2O3
β zeolite is added into iron nitrate aqueous solution, adds silica binder afterwards to form slurry.Slurry is coated in flow type cordierite substrates to obtain 190g/ft3The ferrum load capacity of Fe, dries the base material that Fe/ zeolite is coated with, and then calcines 4 hours 500 DEG C of heating.Then pass through dipping Pd nitrate aqueous solution and palladium is added into the base material of Fe/ zeolite coating to obtain 50g/ft3Pd load capacity, by Pd-Fe/ zeolite be coated with base material dry and 500 DEG C heating and calcine 4 hours.
Platinum nitrate is added into the water slurry of alumina particle (being ground to the diameter particle mean size less than 10 microns) to form Pt/ aluminium oxide catalyst slurry.Then, Pt/ aluminium oxide catalyst slurry is coated on the base material of Pd-Fe/ zeolite coating to obtain 25g/ft3Pt load capacity, and final coating base material is dried, and calcines 4 hours and (comprise 50g/ft 500 DEG C of heating to produce catalyst 1A3Pd, 190g/ft3Fe, and 25g/ft3Pt)。
Catalyst 1B:Pd/ β zeolite+Pt/Al2O3
Program according to comparative catalyst 1A prepares catalyst 1B, except without ferric nitrate.
Embodiment 2: test program
Core product (2.54cmx8.4cm) testing catalytic agent to the cordierite substrates of flow type catalyst coating.Catalyst core first under circulation condition in stove at hydrothermal condition (5%H2O, residual is air) aging 16 hours at 750 DEG C.Then, the feed gas stream prepared by regulating the mass flow of each waste gas component is used to test core catalysis activity in laboratory reaction device.Gas flow rate is maintained at 21.2Lmin-1, obtaining gas hourly space velocity is 30,000h-1(GHSV=30,000h-1)。
Testing catalytic agent under lean-burn condition, uses by 200ppmNO, 200ppmCO, 500ppm decane (with C1Meter), 10%O2, 5%CO2, 5%H2The synthesis waste gas feed stream that O and surplus nitrogen (volume %) form.Catalyst is exposed to feed gas stream, first continues 100 seconds at the isothermal gasinlet temperature of 80 DEG C, and then gasinlet temperature is increased to 650 DEG C with the heating rate of 100 DEG C/min.
It is comparable that the result of table 1 gives catalyst 1B of the present invention and comparative catalyst 1A, it was shown that base metal can remove from the zeolite component of cooled activated catalyst, and does not affect its catalytic performance.
In a word, the cooled activated catalyst system of the present invention shows multiple function, including (1) low temperature NOxStore and be selectively converted to N with height2；(2) low temperature hydrocarbon stores and converts；(3) the CO oxidation activity improved.
The comparison of table 1 catalyst 1B and comparative catalyst 1A.
Catalyst 1B Comparative catalyst 1A*
At 80 DEG C of NOxStorage capacity (g NO2/L) 0.32 0.34
At the last NO of 100 secondsxArresting efficiency (%) 78 78
NO lower than 200 DEG C of accumulationsxStorage capacity (gNO2/L) 0.45 0.46
Store and transformation efficiency (%) lower than the HC of 200 DEG C of accumulations 98 98
CO transformation efficiency (%) lower than 200 DEG C of accumulations 44 45
* comparative example

Claims (16)

1. it is effective in absorption NO below certain low temperaturexWith hydrocarbon (HC) and higher than described low temperature temperature inversion and release absorption NOxWith the cooled activated catalyst of HC, described cooled activated catalyst comprises: the molecular sieve catalyst that (1) is substantially made up of noble metal and molecular sieve；(2) platinum metal catalysts of the load of one or more platinums group metal and one or more inorganic oxide carriers is comprised.
2. cooled activated catalyst according to claim 1, wherein said noble metal is selected from platinum, palladium, rhodium, gold, silver, iridium, ruthenium, osmium and mixture thereof.
3. cooled activated catalyst according to claim 1, wherein said noble metal is palladium.
4. the cooled activated catalyst according to any one of claim 1-3, wherein said molecular sieve is the small pore molecular sieve that maximum loop is of a size of 8 Tetrahedral atoms, maximum loop is of a size of the mesoporous molecular sieve of 10 Tetrahedral atoms, or maximum loop is of a size of the large pore molecular sieve of 12 Tetrahedral atoms.
5. cooled activated catalyst according to claim 4, wherein said molecular sieve has the framing structure selected from AEI, MFI, EMT, ERI, MOR, FER, BEA, FAU, CHA, LEV, MWW, CON, EUO and mixture thereof.
6. the cooled activated catalyst according to any one of claim 1-5, one or more platinums group metal wherein said are selected from platinum, palladium, rhodium, iridium and mixture thereof.
7. the cooled activated catalyst according to any one of claim 1-6, one or more inorganic oxide carriers wherein said are selected from aluminium oxide, silicon dioxide, titanium dioxide, zirconium oxide, ceria, niobium oxide, tantalum pentoxide, molybdenum oxide, tungsten oxide and its mixed oxide or composite oxides.
8. the cooled activated catalyst according to any one of claim 1-7, wherein said cooled activated catalyst is coated on flow type or filtering type base material.
9. cooled activated catalyst according to claim 8, wherein said flow through substrate is honeycomb-type monolith.
10. the cooled activated catalyst according to any one of claim 1-7, wherein described molecular sieve catalyst is extruded to form flow type or filtering type base material, and the platinum metal catalysts of described load is coated on molecular sieve catalyst flow type or the filtering type base material of extrusion.
11. according to the cooled activated catalyst described in any one of claim 1-10, wherein said low temperature is 200 DEG C.
12. the internal combustion engine exhaust system including the cooled activated catalyst according to aforementioned any one of claim.
13. gas extraction system according to claim 12, farther include to be selected from SCR (SCR) catalyst, particulate filter, SCR filter, NOxThe catalyst member of adsorption catalyst, three-way catalyst, oxidation catalyst and combination thereof.
14. the method processing the waste gas from internal combustion engine, described method includes NO lower than certain low temperaturexIt is adsorbed on the cooled activated catalyst described in aforementioned any one of claim with HC, higher than NO from described cooled activated catalyst of the temperature inversion of described low temperature and thermal desorptionxAnd HC, and catalysis removes the NO of desorption on the catalyst member in the downstream of described cooled activated catalystxAnd HC.
15. method according to claim 14, wherein said low temperature is 200 DEG C.
16. according to the method described in claim 14 or claim 15, the catalyst member in the downstream of wherein said cooled activated catalyst is selected from SCR catalyst, particulate filter, SCR filter, NOxAdsorption catalyst, three-way catalyst, oxidation catalyst and combination thereof.
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KR20160096108A (en) 2016-08-12

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